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Title: In-situ incorporation of binder during sol-gel preparation of Pd-based sulfated zirconia for reduction of nitrogen oxides under lean-burn conditions: Effect on activity and wash-coating characteristics

Authors:
; ; ; ;
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1405511
Resource Type:
Journal Article: Publisher's Accepted Manuscript
Journal Name:
Applied Catalysis. B, Environmental
Additional Journal Information:
Journal Volume: 202; Journal Issue: C; Related Information: CHORUS Timestamp: 2017-11-30 13:13:17; Journal ID: ISSN 0926-3373
Publisher:
Elsevier
Country of Publication:
Netherlands
Language:
English

Citation Formats

Sinha Majumdar, Sreshtha, Celik, Gokhan, Alexander, Anne-Marie, Gawade, Preshit, and Ozkan, Umit S. In-situ incorporation of binder during sol-gel preparation of Pd-based sulfated zirconia for reduction of nitrogen oxides under lean-burn conditions: Effect on activity and wash-coating characteristics. Netherlands: N. p., 2017. Web. doi:10.1016/j.apcatb.2016.08.062.
Sinha Majumdar, Sreshtha, Celik, Gokhan, Alexander, Anne-Marie, Gawade, Preshit, & Ozkan, Umit S. In-situ incorporation of binder during sol-gel preparation of Pd-based sulfated zirconia for reduction of nitrogen oxides under lean-burn conditions: Effect on activity and wash-coating characteristics. Netherlands. doi:10.1016/j.apcatb.2016.08.062.
Sinha Majumdar, Sreshtha, Celik, Gokhan, Alexander, Anne-Marie, Gawade, Preshit, and Ozkan, Umit S. Wed . "In-situ incorporation of binder during sol-gel preparation of Pd-based sulfated zirconia for reduction of nitrogen oxides under lean-burn conditions: Effect on activity and wash-coating characteristics". Netherlands. doi:10.1016/j.apcatb.2016.08.062.
@article{osti_1405511,
title = {In-situ incorporation of binder during sol-gel preparation of Pd-based sulfated zirconia for reduction of nitrogen oxides under lean-burn conditions: Effect on activity and wash-coating characteristics},
author = {Sinha Majumdar, Sreshtha and Celik, Gokhan and Alexander, Anne-Marie and Gawade, Preshit and Ozkan, Umit S.},
abstractNote = {},
doi = {10.1016/j.apcatb.2016.08.062},
journal = {Applied Catalysis. B, Environmental},
number = C,
volume = 202,
place = {Netherlands},
year = {Wed Mar 01 00:00:00 EST 2017},
month = {Wed Mar 01 00:00:00 EST 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1016/j.apcatb.2016.08.062

Citation Metrics:
Cited by: 2works
Citation information provided by
Web of Science

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  • The activity and deactivation characteristics of Pt-based lean burn De-NO{sub x} catalysts have been investigated and the relationships between temperature, nature of reductant (n-octane) and NO{sub 2} concentrations, and the mechanism(s) of deactivation have been examined. The effects of Pt loading and particle size on the activity and deactivation have also been studied. The results show that deactivation of the catalyst is due to site blocking via an unidentified carbonaceous deposit and that the initial surface state of the Pt is crucial. In all cases clean Pt surfaces were found to display an initial period of surprisingly high activity priormore » to deactivation, the rate of which was inversely related to reaction temperature. Deactivation is proposed to arise from a combination of factors which inhibit adsorption and reaction of n-octane, due to encroachment onto the Pt surface of hydrocarbonaceous species accumulating initially on the support in the vicinity of the Pt/support interface. It is possible that these carbon-containing deposits comprise some form of organonitrogen species. The loss of activity due to this gradual encroachment results in a reduction in the temperature of the Pt particles, leading to a further decrease in reaction and/or desorption rates, and rapid deactivation then ensues. The use of higher Pt loadings leads to enhanced activity at lower temperatures and increased tolerance to the deactivating effects of surface deposition. Catalyst activity and tolerance to deactivation were further enhanced by controlled sintering, which, within certain limits, resulted in excellent, stable low-temperature De-NO{sub x} activity.« less
  • The kinetics of NO reduction over platinum nanoparticles under lean-burn condition was investigated by first-principles-based kinetic Monte Carlo simulations. Three-dimensional model platinum nanoparticles with diameters ranging from 2.29 to 4.61 nm were represented by a truncated octahedron model consisting of a single (100) facet and eight (111) facets. First-principles density functional theory (DFT) calculations were used to determine the intrinsic kinetic parameters including the binding energies for all of the surface intermediates as well as the activation barriers and reaction energies that comprise the reaction mechanism over the (100) facet, the (111) facet and the (111)/(100) edge sites on themore » three-dimension nanoparticle. Both intra- and inter- facet diffusion of adsorbates were included to model mass transport over the particle surface. The simulation results show that in the presence of excess oxygen, NO reduction to N2 occurs only on the (100) facets. The oxidation of NO to NO2, while much more favored on the (111) facets, can occur on both (100) and (111) facets. Only small amounts of N2O form over the (100) facet. The apparent activation energies for N2 and NO2 formation over the overall particle are 45 kJ/mol and 42 kJ/mol, respectively. This is in agreement with previous experiments. Particle size effects on the activities of NO reduction and oxidation depend on the atomic fractions of the (100) and the (111) facets exposed on the platinum nanoparticles. For the three-dimensional model platinum nanoparticles examined here, the atomic fraction of the (100) facet is nearly the same while the atomic fraction of the (111) facet increases with the increasing particle size. As a result, the activity of NO reduction is insensitive to the particle size. While the larger particle shows higher activity for NO oxidation thus elucidating previous experimental observations. Pacific Northwest National Laboratory is operated by Battelle for the US Department of Energy.« less
  • The catalytic effects of a platinum/aluminium oxide material is described. Temperature and time dependence on the reduction of nitric oxide is discussed.
  • During selective reduction of NO{sub x} under lean-burn conditions, a Pt particle size dependency has previously been observed with various supports. In this study, the authors have examined the influence of various parameters over a large range of initial metal dispersion: nature of the support (silica or alumina), support porosity, presence of impurities (particularly chlorine or sulfur), nature of the platinum precursor salt, and Pt particle size distribution. Furthermore, the authors have considered the mean particle size after sintering under the reactant mixture up to 773 K. Of the factors considered, only the Pt dispersion is of key importance. Themore » intrinsic activity increases with decreasing dispersion (measured initially or after reaction) for each of the main reactions: reduction of NO into N{sub 2} or N{sub 2}O, oxidation of NO into NO{sub 2}, or oxidation of C{sub 3}H{sub 6} into CO{sub 2}. The dispersion does not clearly affect the selectivity.« less
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